Since the discovery of the mesoporous silicate molecular sieve MCM-41 in 1992 the mechanism of formation of organic/inorganic mesostructures in general have been a subject of great interest and debate. This silicate material, and its recently prepared transition metal oxide analogues M-TMS1 (M = Nb, Ta, Ti), consist of a hexagonally-packed array of inorganic tubules ranging from 20-100 in diameter and are formed by templating of inorganic oxides onto a self-assembled liquid crystal mesostructure. These well-defined mesoporous materials are not only of tremendous interest as catalysis or catalytic supports in processes involving large molecules which are unable to diffuse effectively through the smaller microporous channels of zeolites, but also to nanoelectronic devices, host-guest chemistry, and gas sorption processes. We have investigated the structure and dynamics of several transition metal surfactants~in particular, the 15N and 93Nb signals which exhibit lineshape changes due to motional processes.